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    Nitrogen-Doped Carbon Nanotube/Polypropylene Composites with Negative Seebeck Coefficient
    (Basel : MDPI, 2020) Krause, Beate; Konidakis, Ioannis; Arjmand, Mohammad; Sundararaj, Uttandaraman; Fuge, Robert; Liebscher, Marco; Hampel, Silke; Klaus, Maxim; Serpetzoglou, Efthymis; Stratakis, Emmanuel; Pötschke, Petra
    This study describes the application of multi-walled carbon nanotubes that were nitrogen-doped during their synthesis (N-MWCNTs) in melt-mixed polypropylene (PP) composites. Different types of N-MWCNTs, synthesized using different methods, were used and compared. Four of the five MWCNT grades showed negative Seebeck coefficients (S), indicating n-type charge carrier behavior. All prepared composites (with a concentration between 2 and 7.5 wt% N-MWCNTs) also showed negative S values, which in most cases had a higher negative value than the corresponding nanotubes. The S values achieved were between 1.0 µV/K and −13.8 µV/K for the N-MWCNT buckypapers or powders and between −4.7 µV/K and −22.8 µV/K for the corresponding composites. With a higher content of N-MWCNTs, the increase in electrical conductivity led to increasing values of the power factor (PF) despite the unstable behavior of the Seebeck coefficient. The highest power factor was achieved with 4 wt% N-MWCNT, where a suitable combination of high electrical conductivity and acceptable Seebeck coefficient led to a PF value of 6.1 × 10−3 µW/(m·K2). First experiments have shown that transient absorption spectroscopy (TAS) is a useful tool to study the carrier transfer process in CNTs in composites and to correlate it with the Seebeck coefficient.
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    Impact of synthesis temperature on morphology, rheology and electromagnetic interference shielding of CVD-grown carbon nanotube/polyvinylidene fluoride nanocomposites
    (Lausanne : Elsevier Sequoia, 2017) Mirkhani, Seyyed Alireza; Arjmand, Mohammad; Sadeghi, Soheil; Krause, Beate; Pötschke, Petra; Sundararaj, Uttandaraman
    Employing chemical vapor deposition technique, multi-walled carbon nanotubes (CNTs) were synthesized over Fe catalyst at a broad range of temperatures, i.e. 550° C to 950° C (at 100° C intervals). CNTs were melt-mixed into a polyvinylidene fluoride (PVDF) matrix at various loadings, and then compression molded. Surprisingly, despite the ascending trend of CNT powder conductivity with the synthesis temperature, the nanocomposites made with CNT synthesized at 650° C had significantly lower percolation threshold (around 0.4 wt%) and higher electromagnetic interference shielding effectiveness (EMI SE) (20.3 dB over the X-band for 3.5 wt% CNT and 1.1 mm thickness) than the other temperatures. Exhaustive characterization studies were conducted on both CNTs and composites to unveil their morphological and electrical characteristics. Superior EMI shielding of CNT650° C was attributed to a combination of high carbon purity, aspect ratio, crystallinity, and moderate powder conductivity along with decent state of dispersion within the PVDF matrix.
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    Effect of synthesis catalyst on structure of nitrogen-doped carbon nanotubes and electrical conductivity and electromagnetic interference shielding of their polymeric nanocomposites
    (New York, NY [u.a.] : Pergamon Press, 2016) Arjmand, Mohammad; Chizari, Kambiz; Krause, Beate; Pötschke, Petra; Sundararaj, Uttandaraman
    Different catalysts including Co, Fe, and Ni were used to synthesize nitrogen-doped carbon nanotubes (N-CNTs) by chemical vapor deposition technique. Synthesized N-CNTs were melt mixed with a polyvinylidene fluoride (PVDF) matrix using a small scale mixer at different concentrations ranging from 0.3 to 3.5 wt%, and then compression molded. The characterization techniques revealed significant differences in the synthesis yield and the morphological and electrical properties of both N-CNTs and nanocomposites depending on the catalyst type. Whereas Co and Fe resulted in yields comparable to industrial multiwalled CNTs, Ni was much less effective. The N-CNT aspect ratio was the highest for Co catalyst, followed by Ni and Fe, whereas nitrogen content was the highest for Ni. Raman spectroscopy revealed lowest defect number and highest N-CNT crystallinity for Fe catalyst. Characterization of N-CNT/PVDF nanocomposites showed better dispersion for N-CNTs based on Co and Fe as compared to Ni, and the following order of electrical conductivity and electromagnetic interference shielding (from high to low): Co > Fe > Ni. The superior electrical properties of (N-CNT)Co nanocomposites were ascribed to a combination of high synthesis yield, high aspect ratio, low nitrogen content and high crystallinity of N-CNTs combined with a good state of N-CNT dispersion.
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    Tuneable Dielectric Properties Derived from Nitrogen-Doped Carbon Nanotubes in PVDF-Based Nanocomposites
    (Washington, DC : ACS Publications, 2018) Pawar, Shital Patangrao; Arjmand, Mohammad; Pötschke, Petra; Krause, Beate; Fischer, Dieter; Bose, Suryasarathi; Sundararaj, Uttandaraman
    Nitrogen-doped multiwall carbon nanotubes (N-MWNTs) with different structures were synthesized by employing chemical vapor deposition and changing the argon/ethane/nitrogen gas precursor ratio and synthesis time, and broadband dielectric properties of their poly(vinylidene fluoride) (PVDF)-based nanocomposites were investigated. The structure, morphology, and electrical conductivity of synthesized N-MWNTs were assessed via Raman spectroscopy, scanning electron microscopy, transmission electron microscopy, thermogravimetric analysis (TGA), X-ray photoelectron spectroscopy, and powder conductivity techniques. The melt compounded PVDF nanocomposites manifested significantly high real part of the permittivity (ϵ′) along with low dissipation factor (tan δϵ) in 0.1 kHz to 1 MHz frequency range, suggesting use as efficient charge-storage materials. Longer synthesis time resulted in enhanced carbon purity as well as higher thermal stability, determined via TGA analysis. The inherent electrical conductivity of N-MWNTs scaled with the carbon purity. The charge-storage ability of the developed PVDF nanocomposites was commensurate with the amount of the nitrogen heteroatom (i.e., self-polarization), carbon purity, and inherent electrical conductivity of N-MWNTs and increased with better dispersion of N-MWNTs in PVDF.
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    Impact of synthesis temperature on structure of carbon nanotubes and morphological and electrical characterization of their polymeric nanocomposites
    (Melville, NY : AIP, 2017) Arjmand, Mohammad; Mirkhani, Seyyed Alireza; Pötschke, Petra; Krause, Beate; Sundararaj, Uttandaraman
    Carbon nanotubes (CNTs) were synthesized by chemical vapor deposition technique at a broad range of temperatures, i.e. 550°C to 950°C (at 100°C intervals). CNTs were synthesized by flowing source and carrier gases (ethane, argon, and hydrogen) over Fe catalyst in a quartz tubular reactor. CNTs were melt mixed with a polyvinylidene fluoride (PVDF) matrix in a miniature mixer. The resulting nanocomposites were then compression molded, and electrically and morphologically characterized. Moreover, a wide range of characterization techniques were employed to obtain detailed information about the physical and morphological characteristics of CNTs. It was surprisingly observed that, despite the ascending trend of powder conductivity with the synthesis temperature, the nanocomposites made with (CNT)650°C had significantly lower percolation threshold (around 0.4wt.%) and higher electromagnetic interference shielding (20.3dB over the X-band for 1.1mm thickness) compared to the other temperatures. The characterization of nanofillers showed that the synthesis yield and quality of (CNT)650°C were highly superior to the other types of CNTs. At 850°C and 950°C, most of the synthesized carbonaceous materials formed graphitic structures around the sintered catalyst particles. It was also observed that the dispersion state of (CNT)650°C within the PVDF matrix was much better than that of CNTs synthesized at the other temperatures. Superior electrical properties of (CNT)650°C nanocomposites can be attributed to a combination of high synthesis yield, low diameter and decent quality of CNTs coupled with good state of dispersion within the PVDF matrix.